Human sweat has the potential to be sufficiently utilized for noninvasive monitoring. Given the complexity of sweat secretion, the sensitivity and selectivity of sweat monitoring should be further improved. Here, we developed an olfactory-inspired separation-sensing nanochannel-based electronic for sensitive and selective sweat monitoring, which was simultaneously endowed with interferent separation and target detection performances. The special separation-sensing strategy imparts functional composite membranes with a high sensitivity of 113 mV dec–1 for potassium detection. The excellent mechanical properties and conformability of the Kevlar aramid nanofiber layer bring well-wearing performances to realize continuous wireless sweat monitoring. The recognition between functional molecules and target ions is proved at the molecular level in detail in the article. The replacement of functional molecules proves the universality of the strategy for performance enhancement in intricate biofluid analysis systems.
The development of a mass spectrometry-based workflows for monoamine neurotransmitters (NTs) detection in biological samples is crucial for the accurate diagnosis of adrenal tumor. In this study, a carboxyl ionic organic crystal (CIOC) was synthesized via ion self-assembly of cationic and anionic monomers, featuring abundant carboxyl active sites for selective monoamine NTs capture. The CIOC-functionalized paper strips significantly enhance the sensitivity of direct capillary spray miniature mass spectrometry (DCS-mini MS) for monoamine NTs analysis. For biofluid analysis, the CIOC-functionalized paper strips were immersed in samples, washed with ACN to remove interferents, and analyzed by DCS-mini MS. Compared to unmodified paper strips, the CIOC-functionalized paper strips exhibited significantly enhanced sensitivity, with signal amplification factors of 7.6-fold for dopamine, 3.4-fold for norepinephrine, 4.6-fold for 5-hydroxytryptamine, and 5.6-fold for epinephrine in plasma, and corresponding increases of 10.9-fold, 4.0-fold, 6.3-fold, and 7.5-fold in urine. This is attributed to the synergistic effects of electrostatic interactions and hydrogen bonding between CIOC materials and the monoamine NTs. The method showed excellent linearity (R² > 0.9981), with LOD ranging from 0.51 to 2.11 ng mL −1 in urine and 1.53–4.51 ng mL −1 in plasma, and LOQ ranging from 1.7 to 7.01 ng mL −1 in urine and 5.1–15.03 ng mL −1 in plasma. The robustness of the method was confirmed through validation of precision (<10 % RSD) and recoveries (80.1–97.3 %). The CIOC@DCS-mini MS platform enables rapid (3 min), label-free clinical monoamine NTs monitoring, offering a precise solution for diagnosing monoamine NTs-related disorders.
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